The interaction of iron pyrite with oxygen, nitrogen and nitrogen oxides: a first-principles study

Abstract

Sulphide materials, in particular MoS₂, have recently received great attention from the surface science community due to their extraordinary catalytic properties. Interestingly, the chemical activity of iron pyrite (FeS₂) (the most common sulphide mineral on Earth), and in particular its potential for catalytic applications, has not been investigated so thoroughly. In this study, we use density functional theory (DFT) to investigate the surface interactions of fundamental atmospheric components such as oxygen and nitrogen, and we have explored the adsorption and dissociation of nitrogen monoxide (NO) and nitrogen dioxide (NO₂) on the FeS₂(100) surface. Our results show that both those environmentally important NO_x species chemisorb on the surface Fe sites, while the S sites are basically unreactive for all the molecular species considered in this study and even prevent NO₂ adsorption onto one of the non-equivalent Fe–Fe bridge sites of the (1 × 1)–FeS₂(100) surface. From the calculated high barrier for NO and NO₂ direct dissociation on this surface, we can deduce that both nitrogen oxides species are adsorbed molecularly on pyrite surfaces.